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Ultrafast rotational motions of supported nanoclusters probed by electron diffraction

Thomas Vasileiadis, Emmanuel N. Skountzos, Dawn Foster, Shawn P. Coleman, Daniela Zahn, Faruk Krečinić, Vlasis G. Mavrantzas, Richard Palmer Orcid Logo, Ralph Ernstorfer

Nanoscale Horizons, Volume: 4, Issue: 5, Pages: 1164 - 1173

Swansea University Author: Richard Palmer Orcid Logo

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DOI (Published version): 10.1039/C9NH00031C

Abstract

In crystals, microscopic energy flow is governed by electronic and vibrational excitations. In nanoscale materials, however, translations and rotations of entire nanoparticles represent additional fundamental excitations. The observation of such motions is elusive as most ultrafast techniques are in...

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Published in: Nanoscale Horizons
ISSN: 2055-6756 2055-6764
Published: 2019
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URI: https://cronfa.swan.ac.uk/Record/cronfa51706
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spelling 2019-09-06T09:44:58.6183593 v2 51706 2019-09-06 Ultrafast rotational motions of supported nanoclusters probed by electron diffraction 6ae369618efc7424d9774377536ea519 0000-0001-8728-8083 Richard Palmer Richard Palmer true false 2019-09-06 MECH In crystals, microscopic energy flow is governed by electronic and vibrational excitations. In nanoscale materials, however, translations and rotations of entire nanoparticles represent additional fundamental excitations. The observation of such motions is elusive as most ultrafast techniques are insensitive to motions of the phonons’ frame of reference. Here, we study heterostructures of size-selected Au nanoclusters with partial (111) orientation on few-layer graphite with femtosecond electron diffraction. We demonstrate that ultrafast, constrained rotations of nanoclusters, so-called librations, in photo-induced non-equilibrium conditions can be observed separately from vibrational structural dynamics. Molecular dynamics and electron diffraction simulations provide quantitative understanding on librations-induced deviations from the conventional temperature dependence of diffraction patterns. We find that nanocluster librations with a period of ∼20 picoseconds are triggered quasi-impulsively by graphene flexural motions. These ultrafast structural dynamics modulate the Au/C interface and hence are expected to play a key role in energy- and mass-transport at the nanoscale. Journal Article Nanoscale Horizons 4 5 1164 1173 2055-6756 2055-6764 31 12 2019 2019-12-31 10.1039/C9NH00031C COLLEGE NANME Mechanical Engineering COLLEGE CODE MECH Swansea University 2019-09-06T09:44:58.6183593 2019-09-06T09:42:36.6839444 Faculty of Science and Engineering School of Aerospace, Civil, Electrical, General and Mechanical Engineering - Mechanical Engineering Thomas Vasileiadis 1 Emmanuel N. Skountzos 2 Dawn Foster 3 Shawn P. Coleman 4 Daniela Zahn 5 Faruk Krečinić 6 Vlasis G. Mavrantzas 7 Richard Palmer 0000-0001-8728-8083 8 Ralph Ernstorfer 9 0051706-06092019094437.pdf vasileiadis2019.pdf 2019-09-06T09:44:37.1870000 Output 4663505 application/pdf Version of Record true 2019-09-06T00:00:00.0000000 false eng
title Ultrafast rotational motions of supported nanoclusters probed by electron diffraction
spellingShingle Ultrafast rotational motions of supported nanoclusters probed by electron diffraction
Richard Palmer
title_short Ultrafast rotational motions of supported nanoclusters probed by electron diffraction
title_full Ultrafast rotational motions of supported nanoclusters probed by electron diffraction
title_fullStr Ultrafast rotational motions of supported nanoclusters probed by electron diffraction
title_full_unstemmed Ultrafast rotational motions of supported nanoclusters probed by electron diffraction
title_sort Ultrafast rotational motions of supported nanoclusters probed by electron diffraction
author_id_str_mv 6ae369618efc7424d9774377536ea519
author_id_fullname_str_mv 6ae369618efc7424d9774377536ea519_***_Richard Palmer
author Richard Palmer
author2 Thomas Vasileiadis
Emmanuel N. Skountzos
Dawn Foster
Shawn P. Coleman
Daniela Zahn
Faruk Krečinić
Vlasis G. Mavrantzas
Richard Palmer
Ralph Ernstorfer
format Journal article
container_title Nanoscale Horizons
container_volume 4
container_issue 5
container_start_page 1164
publishDate 2019
institution Swansea University
issn 2055-6756
2055-6764
doi_str_mv 10.1039/C9NH00031C
college_str Faculty of Science and Engineering
hierarchytype
hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Aerospace, Civil, Electrical, General and Mechanical Engineering - Mechanical Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Aerospace, Civil, Electrical, General and Mechanical Engineering - Mechanical Engineering
document_store_str 1
active_str 0
description In crystals, microscopic energy flow is governed by electronic and vibrational excitations. In nanoscale materials, however, translations and rotations of entire nanoparticles represent additional fundamental excitations. The observation of such motions is elusive as most ultrafast techniques are insensitive to motions of the phonons’ frame of reference. Here, we study heterostructures of size-selected Au nanoclusters with partial (111) orientation on few-layer graphite with femtosecond electron diffraction. We demonstrate that ultrafast, constrained rotations of nanoclusters, so-called librations, in photo-induced non-equilibrium conditions can be observed separately from vibrational structural dynamics. Molecular dynamics and electron diffraction simulations provide quantitative understanding on librations-induced deviations from the conventional temperature dependence of diffraction patterns. We find that nanocluster librations with a period of ∼20 picoseconds are triggered quasi-impulsively by graphene flexural motions. These ultrafast structural dynamics modulate the Au/C interface and hence are expected to play a key role in energy- and mass-transport at the nanoscale.
published_date 2019-12-31T04:03:43Z
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score 11.013776

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